With a single-atom thickness, excellent electrical conductivity, and superior chemical/electrochemical stability, graphene represents the ideal material for various electrochemical energy storage devices. However, due to the strong π–π interaction between graphene sheets, the graphene flakes tend to re-stack to form graphite-like powders when they are processed into practical electrode materials, which can greatly reduce the specific surface area and lead to inefficient utilization of the graphene layers for electrochemical energy storage. Here I will discuss the assembly of two-dimensional (2D) graphene sheets into three-dimensional holey graphene framework (3D-HGF) structures that can largely retain the unique merits of individual graphene sheets.